Total Collision Cross Sections Research Articles

Dichotomy of the description of the elastic and electronically inelastic scattering of electrons by methane

The interaction between electrons and methane is studied with a particular focus on describing the dynamics of elastic and electronic excitation processes under the influence of the multichannel coupling effects. Elastic and electronically inelastic integral and differential cross sections are reported. These cross sections were calculated with the Schwinger multichannel method implemented with norm-conserving pseudopotentials within the minimal orbital basis for single-configuration interaction approach with up to 181 open channels. While an excellent agreement with previously published data is found in the elastic channel, the comparisons involving electronic excitation cross sections reveal significant discrepancies. Furthermore, the lack of reliable experimental data regarding the electronically inelastic channels hampers a more detailed analysis of the theoretical results. Additionally, total ionization and total cross sections for electron collisions with methane are also presented. By highlighting the current theoretical challenges in dealing with electron-induced electronic excitation of molecules, we seek to contribute to a deeper understanding of this scattering process and, thus, pave the way for future research.

Elastic and electronically inelastic scattering of electrons by the pyrazine molecule.

We report on elastic and electronically inelastic integral and differential cross sections as well as ionization and total cross sections for electron collisions with the pyrazine molecule. The Schwinger multichannel method is applied in calculations carried out according to the minimal orbital basis for single configuration interactions strategy from the 1-channel up to 139-channels close-coupling level of approximation. With these calculations we have obtained integral and differential cross sections as well as excitation functions for elastic electron scattering and, also, integral and differential cross sections for electronic excitation from the ground state to the 3B1u, 3B2u, 3B3u, 1B1u, 1B2u and 1B3u excited states of pyrazine by electron impact. By summing the total ionization cross section obtained by means of the binary-encounter-Bethe model to these elastic and electronically inelastic contributions, we provided an estimate for the total cross section describing the electron-pyrazine interaction process. The independent atom model with the screening-corrected additivity rule plus interference terms method was also used in the present study to determine elastic integral and differential as well as ionization and total cross sections for electron collisions from pyrazine. The present results were, whenever possible, critically compared to the experimental and theoretical data available in the literature. In general, the overall agreement between the present results and the experiment is quite encouraging.

Cross-calibration of atomic pressure sensors and deviation from quantum diffractive collision universality for light particles

The room-temperature, velocity-averaged, total cross section for atom–atom and atom–molecule collisions can be approximated using a universal function depending only on the magnitude of the leading order dispersion coefficient, C 6. This feature of the total cross section together with the universal function for the energy distribution transferred by glancing angle collisions ( (Booth et al 2019 New J. Phys. 21 102001)) can be used to empirically determine the total collision cross section and realize a self-calibrating, vacuum pressure standard. This was previously validated for Rb+N2 and Rb+Rb collisions. However, the post-collision energy distribution is expected to deviate from in the limit of small C 6 and small reduced mass. Here we observe this deviation experimentally by performing a direct cross-species loss rate comparison for Rb+H2 and Li+H2 collisions. We measure a velocity averaged total collision cross section ratio of . Based on an ab initio computation of m3 s−1, we deduce m3 s−1, in agreement with a Rb+H2 ab initio value of . By contrast, fitting the Rb+H2 loss rate as a function of trap depth to the universal function we find m3 s−1. This work demonstrates the utility of sensor-atom cross-calibration experiments to check the validity of theoretical computations to extend and enhance the performance of cold atom based pressure sensors.

Integrated total and state-selective cross sections for bare beryllium ion collisions with atomic hydrogen

We apply the two-centre wave-packet convergent close-coupling approach to calculate integrated total and state-selective cross sections for electron capture and ionisation in bare beryllium ion collisions with atomic hydrogen. This is done in the energy region between 1 keV/u to 1 MeV/u. Good agreement was achieved in comparison to previous theoretical works for the total electron capture cross section across all energies, however the total ionisation cross section shows disagreement with preceding calculations. We present accurate n and ℓ-resolved (n and ℓ are the principal and the angular momentum quantum numbers of the final state in electron capture processes, respectively) cross sections required for plasma impurity diagnostics where there have been discrepancies between different approaches for n > 5. Otherwise, excellent agreement between our results and previous calculations of state-selective cross sections for electron-capture is observed for a wide number of different n. The calculations have been performed on a fine energy mesh to identify oscillatory structures in the n- and nl-resolved capture cross sections in the low-energy region. Our results show pronounced oscillations in the cross sections for n ⩾ 5 below 20 keV/u.

Realization of a universal quantum pressure standard

We report the realization of the first cold-atom primary standard. This standard is based on a universal law governing quantum diffractive collisions between particles that allows an experimental determination of the velocity averaged total collision cross section, the only parameter required to quantify the pressure or flux of particles given a sensor particle collision rate measurement. Using an ensemble of 87Rb sensor atoms, we show that this new quantum pressure standard can be applied to gases of both atomic (He, Ar, and Xe) and molecular species (, , and ), surpassing the scope of existing orifice flow pressure standards. We verify the accuracy of this new standard using an ionization gauge (IG) calibrated for N2 by an orifice flow standard. The gauge calibration factors determined by the cold atom and orifice flow standards differ by less than 0.5% and, thus, agree within their uncertainties of 2% and 2.8% respectively. Using this standard, we evaluate the response of two different IGs to a variety of different gas species and report variations of up to 20% for their measured calibration factors. We also observe a non-linear response of the IG readings for CO2 gas. Finally, we demonstrate the use of a magneto-optical trap (MOT) as a transfer standard to extend the measurement range by a factor of 100 to include pressures up to P ~ 10−5 Pa.

Using Collision Cross Section Distributions to Assess the Distribution of Collision Cross Section Values.

Careful transfer of ions into the gas-phase permits the measurement of protein structures, with ion mobility-mass spectrometry, which provides shape and stoichiometry information. Collision cross sections (CCS) can be obtained from measurements made of the ions mobility through a given gas, and such structural information once obtained should also permit interlaboratory comparisons. However, until recently, there was not a recommended standard form for the reporting of such measurements. In this study, we explore the use of collision cross section distributions to allow comparisons of IM-MS data for commonly analyzed proteins. We present measurements from seven proteins across three IM-MS configurations, namely, an Agilent 6560 IMQToF, a Waters Synapt G2 possessing a TWIMS cell and a modified Synapt G2 possessing an RF confining linear field drift cell. Mobility measurements were taken using He and N2 as the drift gases. To aid comparability across instruments and best assess the corresponding gas-phase conformational landscapes of the protein "standards", we present the data in the form of averaged CCS distributions. For experiments carried out in N2, CCS values for the most compact ion conformations have an interinstrument variability of ≤3%, and the total CCS distributions are generally similar across platforms. For experiments carried out in He, we observe the total CCS distributions to follow the same trend as observed in N2, while CCS for the most compact ion conformations sampled on the 6560 are systematically smaller by up to 10% than those observed on the G2. The calibration procedure (for TWIMS) yields TWCCS for native-like proteins which are largely similar to those obtained on DTIMS instruments. We collate previously reported values of CCS for these proteins in the form of histograms which bear a remarkable similarity to the CCS distributions, reflecting the conformational heterogeneity of proteins and also how conformer populations can be altered on transfer from solution to the detector. This gives concern for some caution when calibrating sample protein drift times simply with single numeric CCS values.

Development of an impulsive model of dissociation in direct simulation Monte Carlo

A previously proposed classical impulsive model for dissociation of diatomic molecules in direct simulation Monte Carlo (DSMC), the Macheret-Fridman for direct simulation Monte Carlo (MF-DSMC) model [Luo et al., “Classical impulsive model for dissociation of diatomic molecules in direct simulation Monte Carlo,” Phys. Rev. Fluids 3, 113401 (2018)], is extended in this work. To improve the prediction of state-specific rates at high vibrational energy, the anharmonic vibrational phase angle distribution function is first incorporated into the model. Then, to improve the prediction of thermal equilibrium dissociation rates, the general concept of calculating total collision cross sections with the MF-DSMC model is discussed and the framework of implementing a collision model based on exponential potential is constructed. The improved model is validated by comparisons with quasiclassical trajectory calculations, empirical estimations, and experimental measurements. In general, better agreement compared with the original version of the model is obtained. The improved model is also evaluated by simulating O2 reacting shock experiment.

CoSIMS: An Optimized Trajectory-Based Collision Simulator for Ion Mobility Spectrometry.

A new, multithreaded, trajectory method based software platform, CoSIMS, is revealed and compared to reference MOBCAL collision cross sections (CCS). CoSIMS employs various molecular mechanics algorithms to lessen the computational resources required to simulate thousands of buffer gas-ion collisions, including the neglect of London dispersion interactions at long distances and the removal of trajectories that insignificantly contribute to the total CCS via an ellipsoidal projection approximation. The showcased program is used to calculate the collision cross sections of carbon fullerenes, proteins, and DNA strands of various lengths, sizes, and molecular weights, and these are compared against the CCSs calculated by MOBCAL. Through this analysis, it is shown that the application of the aforementioned algorithms enables both faster and more reasonable CCS calculations than MOBCAL for highly elongated molecules such as nucleic acids; for all other molecules, CoSIMS is able to reproduce the CCSs generated by MOBCAL's trajectory method within a few percent. Overall, CoSIMS is able to calculate nearly identical CCSs as MOBCAL in nearly 2 orders of magnitude less CPU time due to the various numerical methods implemented into the software, even when run on a single CPU core.

Computation of electron impact scattering studies on benzene

An elaborate theoretical study of electron scattering with benzene over a broad impact energy range is reported in this article. Integrated cross sections such as the electronic excitation cross section, momentum transfer cross section, ionization cross section and the total collision cross section along with the differential elastic cross section are computed at low energy (0.01–20 eV) using ab initio R-matrix employing Quantemol-N. Beyond ionization threshold, the calculations are also carried out using spherical complex optical potential (SCOP) formalism up to 5000 eV. A smooth crossover of the total cross section data is obtained through the two formalisms at the incident energy equal to 13 eV and hence we are able to study the cross sections over a wide energy range. The scattering rate coefficients using the computed elastic cross sections for this target are reported for the first time.

Calculations of Total Classical Cross Sections for a Central Field

In order to find the total collision cross-section a direct method of the effective potential (EPM) in the framework of classical mechanics was proposed. EPM allows to over come both the direct scattering problem (calculation of the total collision cross-section) and the inverse scattering problem (reconstruction of the scattering potential) quickly and effectively. A general analytical expression was proposed for the generalized Lennard-Jones potentials: (6–3), (9–3), (12–3), (6–4), (8–4), (12–4), (8–6), (12–6), (18–6). The values for the scattering potential of the total cross section for pairs such as electron–N $$_{2}$$ , N–N, and O–O $$_{2}$$ were obtained in a good approximation.

Time-dependent microscopic description of total reaction cross sections for collisions of 6He and 9Li nuclei with 28Si nuclei at low and intermediate energies

A microscopic description is given for the collisions of the 9Li and 6He nuclei with the 28Si nucleus. It is based on numerical solution of the time-dependent Schrodinger equation for the external neutrons of the projectile nuclei. The corrections to the nucleus–nucleus potential associated with the redistribution of external neutrons were determined for energies of 5 to 60 MeV/nucleon using the time-dependent folding potential. The probability of leaving the elastic channel was calculated using the reflectionless boundary condition for partial waves. The calculated cross sections are in agreement with the experimental data on the total cross sections for the above reactions.

Entrapment of amino acids in gas phase surfactant assemblies: The case of tryptophan confined in positively charged (1R,2S)-dodecyl (2-hydroxy-1-methyl-2-phenylethyl) dimethylammonium bromide aggregates.

The ability of positively charged aggregates of the surfactant (1R,2S)-dodecyl(2-hydroxy-1-methyl-2-phenylethyl)dimethylammonium bromide (DMEB) to incorporate D-tryptophan or L-tryptophan in the gas phase has been investigated by electrospray ion mobility mass spectrometry (ESI-IM-MS). Strongly impacted by the pH of the electrosprayed solutions, both protonated (T+ ) and deprotonated (T- ) tryptophan are effectively included into the aggregates, whereas, tryptophan in zwitterionic (T0 ) form is practically absent in singly charged DMEB aggregates but can be found in multiply charged ones. The ability to incorporate tryptophan increases with the aggregation number and charge state of aggregates. More than 1 tryptophan species can be entrapped (aggregates including up to 5 tryptophan are observed). Collision induced dissociation experiments performed on the positively singly charged DMEB hexamer containing 1 T- show that at low collision energies the loss of a DMEB molecule is preferred with respect to the loss of the DMEB cation plus T- species which, in turn, is preferred with respect to the loss of mere tryptophan, suggesting that the deprotonated amino acid is preferentially located in proximity of a DMEB head group and with the ionic moiety pointing towards the core of the aggregate. The analysis of the collision cross sections (CCS) of bare and tryptophan containing aggregates allowed evaluating the contributions of tryptophan and bromide ions to the total aggregate CCS. No significant discrimination between D-tryptophan and L-tryptophan by the chiral DMEB aggregates has been evidenced by mass spectra data, CID experiments, and CCS values.

Low-energy and very-low energy total cross sections for electron collisions with N2

Absolute grand total cross sections for electron scattering from N2 are obtained in the energy range from 20 eV down to 5 meV with very narrow electron energy width of 9 meV using the threshold-photoelectron source. Total cross sections obtained in the present study are compared with the previous experimentally obtained results. At the very-low energy region below 50 meV, the present total cross sections are somewhat smaller than those reported by the Aarhus group [S.V. Hoffmann et al., Rev. Sci. Instrum. 73, 4157 (2002)], which has been the only experimental work that provided the total cross sections in the very-low energy region. The energy positions of the peaks in the total cross sections due to the 2 Π g shape resonance are obtained with higher accuracy, due to the improved uncertainty of the energy position in the present measurement compared to the previous works. The resonance structure in the total cross sections due to the Feshbach resonances of N2 at around 11.5 eV are also observed. Analysis of the resonant structure was carried out in order to determine the values of resonance width of Feshbach resonances of N2.

Total single electron capture cross sections for collisions of multicharged ions with He atoms

The three-body boundary corrected Born distorted wave method is utilized to compute the total cross sections for single electron capture in the collisions of the fast ions (, He, Li, and ) with helium targets in their ground states. Both post and prior forms of the transition amplitude are obtained in terms of two-dimensional integrals and the total cross sections are computed via three-dimensional numerical integrations. The present results show reasonable agreement with the measurements and three- and four-body theoretical computations, especially at higher incident energies.

Formation, Fragmentation, and Structures of YxOy(+) (x = 1, 2, y=1-13) Clusters: Collision-Induced Dissociation Experiments and Density Functional Theory Calculations.

Yttrium oxide cluster cations have been experimentally and theoretically studied. We produced small, oxygen-rich yttrium oxide clusters, YxOy+ (x = 1, 2, y = 1–13), by mixing the laser-produced yttrium plasma with a molecular oxygen jet. Mass spectrometry measurements showed that the most stable clusters are those consisting of one yttrium and an odd number of oxygen atoms of the form YO(+)(2k+1) (k = 0–6). Additionally, we performed collision induced dissociation experiments, which indicated that the loss of pairs of oxygen atoms down to a YO+ core is the preferred fragmentation channel for all clusters investigated. Furthermore, we conduct DFT calculations and we obtained two types of low-energy structures: one containing an yttrium cation core and the other composed of YO+ core and O2 ligands, being in agreement with the observed fragmentation pattern. Finally, from the fragmentation studies, total collision cross sections are obtained and these are compared with geometrical cross sections of the calculated structures.

Total cross sections for hadron collisions on the basis of the HPR1R2 model

The results of a quantitative, statistically complete, description of the total-cross-section data obtained worldwide for hadron–hadron (photon–hadron) collisions and compiled in the Particle Data Group surveys are presented for several versions of a universal analytic parametrization of amplitudes for forward hadron–hadron (photon-hadron) scattering.

A study of internal energy relaxation in shocks using molecular dynamics based models

Recent potential energy surfaces (PESs) for the N2 + N and N2 + N2 systems are used in molecular dynamics (MD) to simulate rates of vibrational and rotational relaxations for conditions that occur in hypersonic flows. For both chemical systems, it is found that the rotational relaxation number increases with the translational temperature and decreases as the rotational temperature approaches the translational temperature. The vibrational relaxation number is observed to decrease with translational temperature and approaches the rotational relaxation number in the high temperature region. The rotational and vibrational relaxation numbers are generally larger in the N2 + N2 system. MD-quasi-classical trajectory (QCT) with the PESs is also used to calculate the V-T transition cross sections, the collision cross section, and the dissociation cross section for each collision pair. Direct simulation Monte Carlo (DSMC) results for hypersonic flow over a blunt body with the total collision cross section from MD/QCT simulations, Larsen-Borgnakke with new relaxation numbers, and the N2 dissociation rate from MD/QCT show a profile with a decreased translational temperature and a rotational temperature close to vibrational temperature. The results demonstrate that many of the physical models employed in DSMC should be revised as fundamental potential energy surfaces suitable for high temperature conditions become available.

Total projectile electron loss cross sections ofU28+ions in collisions with gaseous targets ranging from hydrogen to krypton

Beam lifetimes of stored ${\mathrm{U}}^{28+}$ ions with kinetic energies of 30 and $50\text{ }\mathrm{MeV}/\mathrm{u}$, respectively, were measured in the experimental storage ring of the GSI accelerator facility. By using the internal gas target station of the experimental storage ring, it was possible to obtain total projectile electron loss cross sections for collisions with several gaseous targets ranging from hydrogen to krypton from the beam lifetime data. The resulting experimental cross sections are compared to predictions by two theoretical approaches, namely the CTMC method and a combination of the DEPOSIT code and the RICODE program.

A guided-ion beam study of the collisions and reactions of I(+) and I2 (+) with I2.

Growing interest in developing and testing iodine Hall effect thrusters requires measurements of the cross sections of reactions that generate low energy plasma following discharge. Limited experimental and theoretical work necessitates a decisive experiment to elucidate the charge exchange and collision-induced dissociation channels. To this end, we have used guided-ion beam techniques to measure cross sections for both I(+) + I2 and I2 (+)+I2 collisions. We present total collision cross sections as well as collision-induced dissociation cross sections for center-of-mass collision energies ranging from 0.5 to 200 eV for molecular iodine cations. Similarly, we present total collision cross section and charge-exchange cross sections for atomic iodine cations for center-of-mass collision energies ranging from 0.67 to 167 eV. Time-of-flight measurements of the collision products allow determination of velocity distributions, which show evidence of complex formation of I3 (+) from the I(+) + I2 reaction at collision energies below 6 eV.

Nonthermal effects on the elastic electron–atom collision in generalized Lorentzian semiclassical plasmas: Lorentzian renormalization shielding

The Lorentzian renormalization plasma shielding effects on the elastic electron–atom collision are investigated in generalized Lorentzian semiclassical plasmas. The eikonal analysis and the effective interaction potential are employed to obtain the eikonal scattering phase shift, differential eikonal collision cross section, and total eikonal collision cross section as functions of the collision energy, impact parameter, nonthermal renormalization parameter, and spectral index of the Lorentzian plasma. It is found that the influence of Lorentzian renormalization shielding suppresses the eikonal scattering phase shift and, however, enhances the eikonal collision cross section in Lorentzian semiclassical plasmas. Additionally, the energy dependence on the total collision cross section in nonthermal plasmas is found to be more significant than that in thermal plasmas.